Identification of the Origin for Reconstructed Active Sites on Oxyhydroxide for Oxygen Evolution Reaction

© 2022 Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 6 vom: 15. Feb., Seite e2209307
1. Verfasser: Wang, Chen (VerfasserIn)
Weitere Verfasser: Zhai, Panlong, Xia, Mingyue, Liu, Wei, Gao, Junfeng, Sun, Licheng, Hou, Jungang
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2023
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article irreversible reconstruction behavior oxygen evolution reaction oxygen-vacancy-site mechanism reconstruction of active sites transfer of intramolecular electron
Beschreibung
Zusammenfassung:© 2022 Wiley-VCH GmbH.
The regulation of atomic and electronic structures of active sites plays an important role in the rational design of oxygen evolution reaction (OER) catalysts toward electrocatalytic hydrogen generation. However, the precise identification of the active sites for surface reconstruction behavior during OER remains elusive for water-alkali electrolysis. Herein, irreversible reconstruction behavior accompanied by copper dynamic evolution for cobalt iron layered double hydroxide (CoFe LDH) precatalyst to form CoFeCuOOH active species with high-valent Co species is reported, identifying the origin of reconstructed active sites through operando UV-Visible (UV-vis), in situ Raman, and X-ray absorption fine-structure (XAFS) spectroscopies. Density functional theory analysis rationalizes this typical electronic structure evolution causing the transfer of intramolecular electrons to form ligand holes, promoting the reconstruction of active sites. Specifically, unambiguous identification of active sites for CoFeCuOOH is explored by in situ 18 O isotope-labeling differential electrochemical mass spectrometry (DEMS) and supported by theoretical calculation, confirming mechanism switch to oxygen-vacancy-site mechanism (OVSM) pathway on lattice oxygen. This work enables to elucidate the vital role of dynamic active-site generation and the representative contribution of OVSM pathway for efficient OER performance
Beschreibung:Date Completed 10.02.2023
Date Revised 10.02.2023
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202209307